In Situ Electric-Field Control of THz Nonreciprocal Directional Dichroism in the Multiferroic Ba_{2}CoGe_{2}O_{7}.

Nonreciprocal directional dichroism, also called the optical-diode effect, is an appealing functional property inherent to the large class of noncentrosymmetric magnets. However, the in situ electric control of this phenomenon is challenging as it requires a set of conditions to be fulfilled: Special symmetries of the magnetic ground state, spin excitations with comparable magnetic- and electric-dipole activity, and switchable electric polarization. We demonstrate the isothermal electric switch between domains of Ba_{2}CoGe_{2}O_{7} possessing opposite magnetoelectric susceptibilities. Combining THz spectroscopy and multiboson spin-wave analysis, we show that unbalancing the population of antiferromagnetic domains generates the nonreciprocal light absorption of spin excitations.

Giant conductivity of mobile non-oxide domain walls.

Atomically sharp domain walls in ferroelectrics are considered as an ideal platform to realize easy-to-reconfigure nanoelectronic building blocks, created, manipulated and erased by external fields. However, conductive domain walls have been exclusively observed in oxides, where domain wall mobility and conductivity is largely influenced by stoichiometry and defects. Here, we report on giant conductivity of domain walls in the non-oxide ferroelectric GaV4S8. We observe conductive domain walls forming in zig-zagging structures, that are composed of head-to-head and tail-to-tail domain wall segments alternating on the nanoscale. Remarkably, both types of segments possess high conductivity, unimaginable in oxide ferroelectrics. These effectively 2D domain walls, dominating the 3D conductance, can be mobilized by magnetic fields, triggering abrupt conductance changes as large as eight orders of magnitude. These unique properties demonstrate that non-oxide ferroelectrics can be the source of novel phenomena beyond the realm of oxide electronics.

Cooperative Cluster Jahn-Teller Effect as a Possible Route to Antiferroelectricity.

We report the observation of an antipolar phase in cubic GaNb_{4}S_{8} driven by an unconventional microscopic mechanism, the cooperative Jahn-Teller effect of Nb_{4}S_{4} molecular clusters. The assignment of the antipolar nature is based on sudden changes in the crystal structure and a strong drop of the dielectric constant at T_{JT}=31 K, also indicating the first-order nature of the transition. In addition, we found that local symmetry lowering precedes long-range orbital ordering, implying the presence of a dynamic Jahn-Teller effect in the cubic phase above T_{JT}. Based on the variety of structural polymorphs reported in lacunar spinels, also including ferroelectric phases, we argue that GaNb_{4}S_{8} may be transformable to a ferroelectric state, which would further classify the observed antipolar phase as antiferroelectric.

Magneto-optical diagnosis of symptomatic malaria in Papua New Guinea.

Improved methods for malaria diagnosis are urgently needed. Here, we evaluate a novel method named rotating-crystal magneto-optical detection (RMOD) in 956 suspected malaria patients in Papua New Guinea. RMOD tests can be conducted within minutes and at low cost. We systematically evaluate the capability of RMOD to detect infections by directly comparing it with expert light microscopy, rapid diagnostic tests and polymerase chain reaction on capillary blood samples. We show that compared to light microscopy, RMOD exhibits 82% sensitivity and 84% specificity to detect any malaria infection and 87% sensitivity and 88% specificity to detect Plasmodium vivax. This indicates that RMOD could be useful in P. vivax dominated elimination settings. Parasite density correlates well with the quantitative magneto-optical signal. Importantly, residual hemozoin present in malaria-negative patients is also detectable by RMOD, indicating its ability to detect previous infections. This could be exploited to reveal transmission hotspots in low-transmission settings.

Optically Driven Collective Spin Excitations and Magnetization Dynamics in the Néel-type Skyrmion Host GaV_{4}S_{8}.

GaV_{4}S_{8} is a multiferroic semiconductor hosting magnetic cycloid (Cyc) and Néel-type skyrmion lattice (SkL) phases with a broad region of thermal and magnetic stability. Here, we use time-resolved magneto-optical Kerr spectroscopy to show the coherent generation of collective spin excitations in the Cyc and SkL phases. Our micromagnetic simulations reveal that these are driven by an optically induced modulation of uniaxial anisotropy. Our results shed light on spin dynamics in anisotropic materials hosting skyrmions and pave a new pathway for the optical manipulation of their magnetic order.

Microwave Directional Dichroism Resonant with Spin Excitations in the Polar Ferromagnet GaV_{4}S_{8}.

We have investigated the directional dichroism of magnetic resonance spectra in the polar ferromagnet GaV_{4}S_{8}. While four types of structural domains are energetically degenerated under a zero field, the magnetic resonance for each domain is well separated by applying magnetic fields due to uniaxial magnetic anisotropy. Consequently, a directional dichroism as large as 20% is clearly observed without domain cancellation. The present observation therefore demonstrates that not only magnetoelectric monodomain crystals but also magnetoelectric multidomain specimens can be used to realize microwave (optical) diodes owing to the lack of inversion domains.

Magnetic Field Control of Cycloidal Domains and Electric Polarization in Multiferroic BiFeO_{3}.

The magnetic field induced rearrangement of the cycloidal spin structure in ferroelectric monodomain single crystals of the room-temperature multiferroic BiFeO_{3} is studied using small-angle neutron scattering. The cycloid propagation vectors are observed to rotate when magnetic fields applied perpendicular to the rhombohedral (polar) axis exceed a pinning threshold value of ∼5 T. In light of these experimental results, a phenomenological model is proposed that captures the rearrangement of the cycloidal domains, and we revisit the microscopic origin of the magnetoelectric effect. A new coupling between the magnetic anisotropy and the polarization is proposed that explains the recently discovered magnetoelectric polarization perpendicular to the rhombohedral axis.

Equilibrium Skyrmion Lattice Ground State in a Polar Easy-plane Magnet.

The skyrmion lattice state (SkL), a crystal built of mesoscopic spin vortices, gains its stability via thermal fluctuations in all bulk skyrmion host materials known to date. Therefore, its existence is limited to a narrow temperature region below the paramagnetic state. This stability range can drastically increase in systems with restricted geometries, such as thin films, interfaces and nanowires. Thermal quenching can also promote the SkL as a metastable state over extended temperature ranges. Here, we demonstrate more generally that a proper choice of material parameters alone guarantees the thermodynamic stability of the SkL over the full temperature range below the paramagnetic state down to zero kelvin. We found that GaV4Se8, a polar magnet with easy-plane anisotropy, hosts a robust Néel-type SkL even in its ground state. Our supporting theory confirms that polar magnets with weak uniaxial anisotropy are ideal candidates to realize SkLs with wide stability ranges.

Exchange anisotropy in the skyrmion host GaV4S8.

Using ferromagnetic resonance spectroscopy at 34 GHz we explored the magnetic anisotropy of single-crystalline GaV4S8 in the field-polarized magnetic state. We describe the data in terms of an easy-axis type uniaxial anisotropy with an anisotropy constant [Formula: see text] erg cm-3 at 2 K, corresponding to a relative exchange anisotropy [Formula: see text]%, and about [Formula: see text]erg cm-3 near 11 K, i.e. at temperatures where the skyrmion-lattice phase was recently discovered. The relatively large value of K 1 explains the confinement of the skyrmion tubes to the [Formula: see text] easy axes. A distinct set of resonances in the spectra is attributed to the co-existence of different rhombohedral domains. Complementary broadband spectroscopy demonstrates that non-collinear spin states may sensitively be detected by electron spin resonance techniques.

Polar Dynamics at the Jahn-Teller Transition in Ferroelectric GaV4S8.

We present a dielectric spectroscopy study of the polar dynamics linked to the orbitally driven ferroelectric transition in the Skyrmion host GaV(4)S(8). By combining THz and MHz-GHz spectroscopy techniques, we succeed in detecting the relaxational dynamics arising from coupled orbital and polar fluctuations in this material and trace its temperature dependence in the paraelectric as well as in the ferroelectric phase. The relaxation time significantly increases when approaching the critical temperature from both sides of the transition. It is natural to assume that these polar fluctuations map the orbital dynamics at the Jahn-Teller transition. Because of the first-order character of the orbital-ordering transition, the relaxation time shows an enormous jump of about 5 orders of magnitude at the polar and structural phase transition.

Optical Diode Effect at Spin-Wave Excitations of the Room-Temperature Multiferroic BiFeO_{3}.

Multiferroics permit the magnetic control of the electric polarization and the electric control of the magnetization. These static magnetoelectric (ME) effects are of enormous interest: The ability to read and write a magnetic state current-free by an electric voltage would provide a huge technological advantage. Dynamic or optical ME effects are equally interesting, because they give rise to unidirectional light propagation as recently observed in low-temperature multiferroics. This phenomenon, if realized at room temperature, would allow the development of optical diodes which transmit unpolarized light in one, but not in the opposite, direction. Here, we report strong unidirectional transmission in the room-temperature multiferroic BiFeO_{3} over the gigahertz-terahertz frequency range. The supporting theory attributes the observed unidirectional transmission to the spin-current-driven dynamic ME effect. These findings are an important step toward the realization of optical diodes, supplemented by the ability to switch the transmission direction with a magnetic or electric field.

Néel-type skyrmion lattice with confined orientation in the polar magnetic semiconductor GaV4S8.

Following the early prediction of the skyrmion lattice (SkL)--a periodic array of spin vortices--it has been observed recently in various magnetic crystals mostly with chiral structure. Although non-chiral but polar crystals with Cnv symmetry were identified as ideal SkL hosts in pioneering theoretical studies, this archetype of SkL has remained experimentally unexplored. Here, we report the discovery of a SkL in the polar magnetic semiconductor GaV4S8 with rhombohedral (C3v) symmetry and easy axis anisotropy. The SkL exists over an unusually broad temperature range compared with other bulk crystals and the orientation of the vortices is not controlled by the external magnetic field, but instead confined to the magnetic easy axis. Supporting theory attributes these unique features to a new Néel-type of SkL describable as a superposition of spin cycloids in contrast to the Bloch-type SkL in chiral magnets described in terms of spin helices.

One-way transparency of four-coloured spin-wave excitations in multiferroic materials.

The coupling between spins and electric dipoles governs magnetoelectric phenomena in multiferroics. The dynamical magnetoelectric effect, which is an inherent attribute of the spin excitations in multiferroics, drastically changes the optical properties of these compounds compared with conventional materials where light-matter interaction is expressed only by the dielectric permittivity or magnetic permeability. Here we show via polarized terahertz spectroscopy studies on multiferroic Ca2CoSi2O7, Sr2CoSi2O7 and Ba2CoGe2O7 that such magnetoeletric spin excitations exhibit quadrochroism, that is, they have different colours for all the four combinations of the two propagation directions (forward or backward) and the two orthogonal polarizations of a light beam. We demonstrate that one-way transparency can be realized for spin-wave excitations with sufficiently strong optical magnetoelectric effect. Furthermore, the transparent and absorbing directions of light propagation can be reversed by external magnetic fields. This magnetically controlled optical-diode function of magnetoelectric multiferroics may open a new horizon in photonics.

Malaria pigment crystals as magnetic micro-rotors: key for high-sensitivity diagnosis.

The need to develop new methods for the high-sensitivity diagnosis of malaria has initiated a global activity in medical and interdisciplinary sciences. Most of the diverse variety of emerging techniques are based on research-grade instruments, sophisticated reagent-based assays or rely on expertise. Here, we suggest an alternative optical methodology with an easy-to-use and cost-effective instrumentation based on unique properties of malaria pigment reported previously and determined quantitatively in the present study. Malaria pigment, also called hemozoin, is an insoluble microcrystalline form of heme. These crystallites show remarkable magnetic and optical anisotropy distinctly from any other components of blood. As a consequence, they can simultaneously act as magnetically driven micro-rotors and spinning polarizers in suspensions. These properties can gain importance not only in malaria diagnosis and therapies, where hemozoin is considered as drug target or immune modulator, but also in the magnetic manipulation of cells and tissues on the microscopic scale.

Enhanced infrared magneto-optical response of the nonmagnetic semiconductor BiTeI driven by bulk Rashba splitting.

We study the magneto-optical (MO) response of the polar semiconductor BiTeI with giant bulk Rashba spin splitting at various carrier densities. Despite being nonmagnetic, the material is found to yield a huge MO activity in the infrared region under moderate magnetic fields (up to 3 T). Our first-principles calculations show that the enhanced MO response of BiTeI comes mainly from the intraband transitions between the Rashba-split bulk conduction bands. These transitions connecting electronic states with opposite spin directions become active due to the presence of strong spin-orbit interaction and give rise to distinct features in the MO spectra with a systematic doping dependence. We predict an even more pronounced enhancement in the low-energy MO response and dc Hall effect near the crossing (Dirac) point of the conduction bands.

Spin-stretching modes in anisotropic magnets: spin-wave excitations in the multiferroic Ba2CoGe2O7.

We studied spin excitations in the magnetically ordered phase of the noncentrosymmetric Ba(2)CoGe(2)O(7) in high magnetic fields up to 33 T. In the electron spin resonance and far infrared absorption spectra we found several spin excitations beyond the two conventional magnon modes expected for such a two-sublattice antiferromagnet. We show that a multiboson spin-wave theory describes these unconventional modes, including spin-stretching modes, characterized by an oscillating magnetic dipole and quadrupole moment. The lack of inversion symmetry allows each mode to become electric dipole active. We expect that the spin-stretching modes can be generally observed in inelastic neutron scattering and light absorption experiments in a broad class of ordered S > 1/2 spin systems with strong single-ion anisotropy and/or noncentrosymmetric lattice structure.

Disorder promotes ferromagnetism: rounding of the quantum phase transition in Sr(1-x)Ca(x)RuO3.

The subtle interplay of randomness and quantum fluctuations at low temperatures gives rise to a plethora of unconventional phenomena in systems ranging from quantum magnets and correlated electron materials to ultracold atomic gases. Particularly strong disorder effects have been predicted to occur at zero-temperature quantum phase transitions. Here, we demonstrate that the composition-driven ferromagnetic-to-paramagnetic quantum phase transition in Sr(1-x)Ca(x)RuO3 is completely destroyed by the disorder introduced via the different ionic radii of the randomly distributed Sr and Ca ions. Using a magneto-optical technique, we map the magnetic phase diagram in the composition-temperature space. We find that the ferromagnetic phase is significantly extended by the disorder and develops a pronounced tail over a broad range of the composition x. These findings are explained by a microscopic model of smeared quantum phase transitions in itinerant magnets. Moreover, our theoretical study implies that correlated disorder is even more powerful in promoting ferromagnetism than random disorder.

Enhanced directional dichroism of terahertz light in resonance with magnetic excitations of the multiferroic Ba2CoGe2O7 oxide compound.

We propose that concurrently magnetic and ferroelectric, i.e., multiferroic, compounds endowed with electrically active magnetic excitations (electromagnons) provide a key to producing large directional dichroism for long wavelengths of light. By exploiting the control of ferroelectric polarization and magnetization in a multiferroic oxide Ba(2)CoGe(2)O(7), we demonstrate the realization of such a directional light-switch function at terahertz frequencies in resonance with the electromagnon absorption. Our results imply that this hidden potential is present in a broad variety of multiferroics.

Magnetic-order-induced crystal symmetry lowering in ACr2O4 ferrimagnetic spinels.

We demonstrate that the onset of complex spin orders in ACr2O4 spinels with magnetic and Jahn-Teller active A=Fe and Cu ions lowers the lattice symmetry. This is clearly indicated by the emergence of anisotropic lattice dynamics-i.e., by the pronounced phonon splittings-even when experiments probing static distortions fail. The crystal symmetry in the magnetic phase is reduced from tetragonal to orthorhombic for both compounds. The conical spin ordering in FeCr2O4 is also manifested in the hardening of the phonon frequencies. In contrast, the multiferroic CoCr2O4 with no orbital degrees of freedom shows tiny deviations from cubic structure even in its ground state.

Optical probe for anomalous Hall resonance in ferromagnets with spin chirality.

We have investigated the infrared optical Hall conductivity, sigma(xy)(omega) for band-filling-controlled ferromagnetic crystals of Nd2Mo2O7, revealing the dynamical properties of their anomalous Hall effect (AHE). A resonant structure and its systematic filling dependence were observed in the Hall conductivity spectra in the midinfrared region (typically at 0.1 eV), while similar effects were not discerned in the diagonal (longitudinal or ordinary) conductivity spectra. This property of sigma(xy)(omega) provides crucial and essential information to understand the microscopic mechanism of AHE including its dc limit. Specifically, the interband transition at the magnetic-monopole-like band-anticrossing point, which is split by spin chirality, is the dominant source in AHE.